CN113039666B - Electrode paste coating apparatus and method for forming dual active material layer - Google Patents

Electrode paste coating apparatus and method for forming dual active material layer Download PDF

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Publication number
CN113039666B
CN113039666B CN202080005130.8A CN202080005130A CN113039666B CN 113039666 B CN113039666 B CN 113039666B CN 202080005130 A CN202080005130 A CN 202080005130A CN 113039666 B CN113039666 B CN 113039666B
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slurry
layer
coating
discharge port
discharge
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CN113039666A (en
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李泽秀
曺永俊
崔相勳
金寄泰
尹智熙
金哲佑
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LG Energy Solution Ltd
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LG Chem Ltd
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C—APPARATUS FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C5/00—Apparatus in which liquid or other fluent material is projected, poured or allowed to flow on to the surface of the work
    • B05C5/02—Apparatus in which liquid or other fluent material is projected, poured or allowed to flow on to the surface of the work the liquid or other fluent material being discharged through an outlet orifice by pressure, e.g. from an outlet device in contact or almost in contact, with the work
    • B05C5/0254—Coating heads with slot-shaped outlet
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C—APPARATUS FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C5/00—Apparatus in which liquid or other fluent material is projected, poured or allowed to flow on to the surface of the work
    • B05C5/02—Apparatus in which liquid or other fluent material is projected, poured or allowed to flow on to the surface of the work the liquid or other fluent material being discharged through an outlet orifice by pressure, e.g. from an outlet device in contact or almost in contact, with the work
    • B05C5/0254—Coating heads with slot-shaped outlet
    • B05C5/0258—Coating heads with slot-shaped outlet flow controlled, e.g. by a valve
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C—APPARATUS FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C5/00—Apparatus in which liquid or other fluent material is projected, poured or allowed to flow on to the surface of the work
    • B05C5/02—Apparatus in which liquid or other fluent material is projected, poured or allowed to flow on to the surface of the work the liquid or other fluent material being discharged through an outlet orifice by pressure, e.g. from an outlet device in contact or almost in contact, with the work
    • B05C5/027—Coating heads with several outlets, e.g. aligned transversally to the moving direction of a web to be coated
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C—APPARATUS FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C11/00—Component parts, details or accessories not specifically provided for in groups B05C1/00 - B05C9/00
    • B05C11/10—Storage, supply or control of liquid or other fluent material; Recovery of excess liquid or other fluent material
    • B05C11/1002—Means for controlling supply, i.e. flow or pressure, of liquid or other fluent material to the applying apparatus, e.g. valves
    • B05C11/1005—Means for controlling supply, i.e. flow or pressure, of liquid or other fluent material to the applying apparatus, e.g. valves responsive to condition of liquid or other fluent material already applied to the surface, e.g. coating thickness, weight or pattern
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C—APPARATUS FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C11/00—Component parts, details or accessories not specifically provided for in groups B05C1/00 - B05C9/00
    • B05C11/10—Storage, supply or control of liquid or other fluent material; Recovery of excess liquid or other fluent material
    • B05C11/1002—Means for controlling supply, i.e. flow or pressure, of liquid or other fluent material to the applying apparatus, e.g. valves
    • B05C11/1015—Means for controlling supply, i.e. flow or pressure, of liquid or other fluent material to the applying apparatus, e.g. valves responsive to a conditions of ambient medium or target, e.g. humidity, temperature ; responsive to position or movement of the coating head relative to the target
    • B05C11/1018—Means for controlling supply, i.e. flow or pressure, of liquid or other fluent material to the applying apparatus, e.g. valves responsive to a conditions of ambient medium or target, e.g. humidity, temperature ; responsive to position or movement of the coating head relative to the target responsive to distance of target
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C—APPARATUS FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C5/00—Apparatus in which liquid or other fluent material is projected, poured or allowed to flow on to the surface of the work
    • B05C5/02—Apparatus in which liquid or other fluent material is projected, poured or allowed to flow on to the surface of the work the liquid or other fluent material being discharged through an outlet orifice by pressure, e.g. from an outlet device in contact or almost in contact, with the work
    • B05C5/027—Coating heads with several outlets, e.g. aligned transversally to the moving direction of a web to be coated
    • B05C5/0275—Coating heads with several outlets, e.g. aligned transversally to the moving direction of a web to be coated flow controlled, e.g. by a valve
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C—APPARATUS FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05C9/00—Apparatus or plant for applying liquid or other fluent material to surfaces by means not covered by any preceding group, or in which the means of applying the liquid or other fluent material is not important
    • B05C9/06—Apparatus or plant for applying liquid or other fluent material to surfaces by means not covered by any preceding group, or in which the means of applying the liquid or other fluent material is not important for applying two different liquids or other fluent materials, or the same liquid or other fluent material twice, to the same side of the work
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05D—PROCESSES FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
    • B05D1/00—Processes for applying liquids or other fluent materials
    • B05D1/26—Processes for applying liquids or other fluent materials performed by applying the liquid or other fluent material from an outlet device in contact with, or almost in contact with, the surface
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0404—Methods of deposition of the material by coating on electrode collectors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0409—Methods of deposition of the material by a doctor blade method, slip-casting or roller coating
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The present invention relates to an electrode paste coating apparatus and method which ultimately allows for improved process efficiency and reduced error rate in forming a two-layer structured active material layer by temporarily adjusting the heights of a first discharge port and a second discharge port through which active material is discharged.

Description

Electrode paste coating apparatus and method for forming dual active material layer
Technical Field
This application claims the benefit of priority from korean patent application No. 10-2019-0128891, filed on 17.10.2019, the entire disclosure of which is incorporated herein by reference.
The present invention relates to an electrode paste coating apparatus and method for forming an active material layer having a double-layer structure.
Background
As technology develops and the demand for mobile devices increases, the demand for secondary batteries also rapidly increases. Among them, lithium secondary batteries are widely used as energy sources for various electronic products and various mobile devices due to their high energy density and high operating voltage as well as excellent storage and life characteristics.
In addition, as a solution to air pollution of existing gasoline automobiles and diesel automobiles using fossil fuels, secondary batteries are attracting attention as energy sources for electric automobiles, hybrid automobiles, and the like. In order to be used as a power source for electric vehicles, a high-power battery is required.
In order to improve the performance of the secondary battery, the development of an electrode structure in which an active material layer having a two-layer structure is formed on a current collector has attracted attention. A method of forming two active material layers on a current collector is to sequentially coat a slurry forming a lower active material layer and an upper active material layer on the current collector in the form of a thin metal film. However, when the slurry forming the lower active material layer and the upper active material layer is discharged at one time, the lower active material and the upper active material are mixed with each other, so that a desired double-layer structure cannot be formed.
Therefore, when manufacturing an electrode having an active material of a double-layer structure, it is required to develop a technique capable of efficiently forming an active material layer having a double-layer structure in an electrode paste coating process.
Disclosure of Invention
Technical problem
The present invention has been made to solve the above-mentioned problems, and it is an object of the present invention to provide an electrode paste coating apparatus and method for forming an active material layer having a double-layer structure with improved process efficiency.
Technical scheme
An electrode paste coating apparatus 130 according to the present invention is composed of a lower plate 131, a middle plate 132, and an upper plate 133, the apparatus including: a first discharge port 110 formed between the lower plate 131 and the middle plate 132, for discharging the slurry forming the lower slurry layer onto the current collector; a second discharge port 120 formed between the middle plate 132 and the upper plate 133, positioned to be spaced apart from the first discharge port downstream in a coating direction, and for discharging slurry forming an upper slurry layer onto the lower slurry layer on the current collector; and a movement controller for moving the coating apparatus in a direction opposite to the discharging direction.
In the present invention, the end portions of the lower plate, the middle plate, and the upper plate are located on the same line.
In one embodiment, the movement controller controls the shortest distance H1 between the end of the coating apparatus and the current collector to satisfy the following condition:
[ Condition ]
When a certain time has elapsed after the formation of the lower slurry layer, the apparatus is moved in the direction opposite to the discharging direction to form an upper slurry layer on the lower slurry layer, at which time the apparatus is moved by a distance H1 T In the range of 60% to 140% of the average thickness of the sizing layer.
If the above range is less than 60%, the space where the slurry stays for coating, that is, the total area between the end of the coating apparatus and the lower slurry layer is insufficient compared to the amount of discharged liquid, and thus the supplied slurry cannot be coated to leak back. On the other hand, in the case of more than 140%, the coating area is too large compared to the supplied slurry, resulting in that the coating cannot be performed uniformly, or only the lower layer and not the upper layer can be coated.
In another example, a point of time at which the coating apparatus moves in a direction opposite to the discharging direction is calculated by the following formula 1:
[ equation 1]
Moving switching point (T) dS Sec (thickness of the intermediate plate (a) (mm) + thickness of the first discharge port (b) (mm))/moving speed of the current collector in the Moving Direction (MD) (mm/sec).
In a specific example, the shortest distance between the end of the apparatus and the current collector before the start of electrode slurry coating (H1) S ) In the range of 60% to 140% of the average thickness of the lower slurry layer.
If the above range is less than 60%, the space where the slurry stays for coating, that is, the total area between the end of the coating apparatus and the current collector is insufficient compared to the amount of discharged liquid, and thus the supplied slurry cannot be coated to leak back. On the other hand, when exceeding 140%, the coating area becomes too large compared to the supplied slurry, resulting in a phenomenon in which coating is performed unevenly.
Further, the average thickness of each of the upper slurry layer and the lower slurry layer is 40 μm to 200 μm.
Typically, the average particle size of the secondary battery active material is about 10 μm, but since the particle size follows a normal distribution, d (90) or d (max) is typically greater than 10 μm. In order to obtain good coating, in the present invention, the coating apparatus is moved in the direction opposite to the discharge direction to form the upper slurry layer. At this time, when the average thickness of the sizing layer is less than 40 μm, the moving distance H1 T At a value between 24 μm and 56 μm. In this case, as the distance H1 is moved T Becomes close to d (max) and moves a distance H1 when the active material is applied T And active material having the largest particle size become close, and when the active material contained in the coating slurry is coated, it may occur that the particle size of H1 cannot be exceeded T The same height. This may cause defects on the coating surface, for example, lines are formed on the coating surface due to the entrapment of large active materials, and the large active materials are entrapped between the moving current collector and the coating end and damage the current collector, thus causing a cracking phenomenon of the current collector.
Further, it may be advantageous if the thickness of the slurry layer is 200 μm or more, but there is a problem in that it is difficult to practically realize a coating amount exceeding 200 μm that is practically used for the secondary battery.
In addition, the present invention further comprises: a first valve configured to open and close discharge of the first discharge port; a second valve configured to open and close discharge of the second discharge port; and a valve controller configured to control opening and closing of the first valve and the second valve.
In a specific example, at the end of the electrode paste application, the valve controller sets the closing time of the second valve to be delayed from the closing time of the first valve by a closing delay time according to the following equation 2:
[ formula 2]
Sizing discharge off delay time (T) dT Sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD).
For example, the electrode paste coating apparatus is a positive electrode paste coating apparatus for a secondary battery.
The present invention also provides an electrode paste coating method using the electrode paste coating apparatus as described above.
The method of coating an electrode paste according to the present invention comprises the steps of: forming a lower slurry layer by discharging slurry through a first discharge port onto a current collector moving in a coating direction (MD) by using an apparatus 130 for coating electrode slurry composed of a lower plate 131, an intermediate plate 132, and an upper plate 133; moving the apparatus in a direction opposite to the discharge direction; and forming an upper slurry layer by discharging the slurry through a second discharge port onto the lower slurry layer, the second discharge port being positioned spaced apart from the first discharge port downstream in the coating direction, wherein end portions of the lower plate, the middle plate, and the upper plate are located on the same line.
In one example, a point of time at which the coating apparatus moves in a direction opposite to the discharging direction is calculated by the following formula 1:
[ equation 1]
Moving the switching point (T) dS Sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD)).
In another specific example, according to the electrode paste coating method of the present invention, when the electrode paste is coated, the discharge of the paste through the first discharge port is started, and when the coating apparatus is moved in the direction opposite to the discharge direction, the discharge of the paste through the second discharge port is started.
For example, the end of the apparatus and the electrode slurry coating start beforeThe shortest distance between the current collectors (H1) S ) In the range of 60% to 140% of the average thickness of the lower slurry layer.
If the above range is less than 60%, the space where the slurry stays for coating, that is, the total area between the end of the coating apparatus and the current collector is insufficient compared to the amount of discharged liquid, and thus the supplied slurry cannot be coated to leak back. On the other hand, in the case of more than 140%, the coating area is too large compared to the supplied slurry, resulting in a phenomenon that the coating cannot be performed uniformly.
In another example, the electrode paste coating method according to the present invention is characterized in that, at the end of electrode paste coating, the discharge stop time of the paste forming the upper paste layer is delayed from the discharge stop time of the paste forming the lower paste layer by a closing delay time according to the following formula 2:
[ formula 2]
Sizing discharge off delay time (T) dT Sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD).
Further, according to the discharge delay of the present invention, the difference in distance between the coating end point of the upper slurry layer and the coating end point of the lower slurry layer is preferably within 3 mm.
Furthermore, the average thickness (D) of the lower slurry layer of the present invention 1 ) And the average thickness (D) of the sizing layer 2 ) The ratio of 1: 3 to 3: 1.
the thickness of the slurry layer as described above can be regarded as the pressure of the slurry supplied immediately. When the pressure of supplying the upper slurry layer exceeds 3 times of the pressure of the lower slurry layer, the ratio of the thickness of the lower slurry layer to the thickness of the upper slurry layer is 1: 3 or more, since the upper layer has a higher pressure than the lower layer, the lower layer slurry may be pushed back in a direction opposite to the coating direction, thereby increasing the possibility of leakage, and the lower slurry may not be properly supplied due to the high pressure of the upper slurry. Further, due to the high pressure of the upper slurry, the slurry supply to the lower slurry layer is not uniform, and thus it is difficult to form the lower slurry layer uniformly.
On the other hand, when the pressure of supplying the lower slurry layer exceeds the pressure of the upper slurry layer by 3 times, the ratio of the thicknesses of the lower slurry layer and the upper slurry layer is 3: 1 or more, there is a problem that the supply of the sizing layer becomes difficult, or the coating of the sizing layer may be pushed in the coating direction and the surface of the coating liquid may be uneven.
Advantageous effects
The electrode slurry coating apparatus and method according to the present invention may improve process efficiency and reduce a defect rate when forming an active material layer having a double-layered structure on a current collector. In addition, the electrode area discarded after the process can be reduced by reducing the divided section.
Drawings
Fig. 1 is a schematic view illustrating an active material paste coating process using an electrode paste coating apparatus according to an embodiment of the present invention.
Fig. 2 is a schematic view illustrating an electrode paste coating method according to an embodiment of the present invention.
Fig. 3 is a schematic view illustrating a cross-section of an electrode manufactured according to an electrode paste coating method according to an embodiment of the present invention.
Detailed Description
Hereinafter, the present invention will be described in detail with reference to the accompanying drawings. The terms and words used in the present specification and claims should not be construed as being limited to general or dictionary terms, and the inventor can appropriately define the concept of the terms to best describe the invention. The terms and words should be interpreted as meanings and concepts consistent with the technical idea of the present invention.
In the present invention, "coating completion" refers not only to a case where the electrode slurry coating is terminated but also to a case where the slurry coating is temporarily stopped. Specifically, it includes a case where the operation of the electrode paste application apparatus is terminated or temporarily stopped, for example, a case where the paste application is repeated and interrupted to form a patterned active material layer, and a case where the paste application is stopped.
In the present invention, "start of coating" includes not only the case of starting the electrode slurry coating but also the case of resuming the slurry coating that was temporarily stopped. Specifically, it includes a case where the operation of the electrode paste application apparatus is started or the operation that has been temporarily stopped is restarted, for example, a case where the paste application is repeated and interrupted to form a patterned active material layer, and a case where the paste application is performed.
In addition, in the present invention, "corresponding" of two specific points is meant to include a case where two points are located on the same line or within a similar range thereof. The fact that two points are located on the same line includes not only the case where they are physically located on the same line but also the case where they exist within an error range of a facility or a measuring apparatus or a range including a buffer area of a certain level.
Generally, in manufacturing an electrode, a slurry including an active material, a conductive material, and a binder is prepared, the slurry is discharged onto a current collector to form a slurry layer, and finally, an active material layer (electrode layer) is formed through a drying process.
The present invention relates to an electrode paste coating apparatus and method for manufacturing an electrode having a double-layered active material layer.
First, the present invention relates to an electrode paste coating apparatus 130 composed of a lower plate 131, an intermediate plate 132, and an upper plate 133, the apparatus including: a first discharge port 110 formed between the lower plate 131 and the middle plate 132, and for discharging the slurry forming the lower slurry layer onto the current collector; a second discharge port 120 formed between the middle plate 132 and the upper plate 133, positioned to be spaced apart from the first discharge port downstream in the coating direction, and for discharging the slurry forming the upper slurry layer onto the lower slurry layer on the current collector; and a movement controller for moving the coating apparatus in a direction opposite to the discharging direction.
The present invention is characterized in that the ends of the lower plate, the middle plate and the upper plate are positioned on the same line.
In one embodiment, the moving controller moves the electrode slurry coating apparatus such that the shortest distance H1 between the end of the coating apparatus and the current collector satisfies the following condition:
[ Condition ]
When a certain time has elapsed after the formation of the lower slurry layer, the coating apparatus is moved in the direction opposite to the discharge direction, thereby forming an upper slurry layer on the lower slurry layer. At this time, the movement distance H1 T In the range of 60% to 140% of the average thickness of the upper slurry layer. Preferably, H1 T In the range of 60% to 120% or 60% to 100% of the average thickness of the upper slurry layer. H1 T Providing space for forming the sizing layer.
If the above range is less than 60%, the space where the slurry stays for coating, that is, the total area between the end of the coating apparatus and the lower slurry layer is insufficient compared to the amount of discharged liquid, and thus the supplied slurry cannot be coated to leak back. On the other hand, in the case of more than 140%, the coating area is too large compared to the supplied slurry, and thus the coating layer cannot be uniformly applied, or only the lower layer and not the upper layer may be applied.
Therefore, in the electrode paste coating apparatus according to the present invention, the lower paste layer and the upper paste layer are not mixed, and then the lower paste layer and the upper paste layer are dried to stably form a two-layer structure composed of the lower active material layer and the upper active material layer.
In the present invention, the average thickness of the upper slurry layer is preferably 40 μm to 200 μm, more preferably 50 μm to 180 μm, and the average thickness of the lower slurry layer is 40 μm to 200 μm, more preferably 50 μm to 180 μm.
Typically, the average particle size of the secondary battery active material is about 10 μm, but since the particle size follows a normal distribution, d (90) or d (max) is typically greater than 10 μm. In order to obtain good coating, in the present invention, the coating apparatus is moved in the direction opposite to the discharge direction to form the upper slurry layer. At this time, when the average thickness of the sizing layer is less than 40 μm, the moving distance H1 T At a value between 24 μm and 56 μm. In this case, as the distance H1 is moved T Becomes close to d (max) and moves a distance H1 when coated with an active material T And active material having the largest particle size, and when the active material contained in the coating slurry is coated, it may occur that the particle size of H1 cannot be exceeded T The same height.This is because it may cause defects on the coating surface, for example, lines are formed on the coating surface due to the entrapment of large active materials, and the large active materials are entrapped between the moving current collector and the coating end and damage the current collector, thus causing a cracking phenomenon of the current collector.
Further, it may be advantageous if the thickness of the slurry layer is 200 μm or more, but there is a problem in that it is difficult to practically realize a coating amount exceeding 200 μm that is practically used for the secondary battery.
Further, the time point at which the coating apparatus moves in the direction opposite to the discharging direction can be calculated, for example, by the following formula 1:
[ equation 1]
Moving the switching point (T) dS Sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD)).
In the electrode slurry coating apparatus according to the present invention, the shortest distance between the end of the coating apparatus and the current collector, i.e., the height H1, is changed from H1 after the position (movement) change time calculated by the above formula S Variation H1 T . Here, the shortest distance between the end of the coating apparatus and the current collector means a length from straight ends of the upper, middle and lower plates of the coating apparatus to a vertical tangent of the current collector.
This is to stably form an upper paste layer on a lower paste layer formed after the lower paste layer is first formed.
In one example, the shortest distance between the current collector and the end of the coating apparatus before the start of electrode slurry coating (H1) S ) Is controlled in the range of 60% to 140%, preferably 80% to 120%, more preferably 80% to 100% of the average thickness of the lower slurry layer.
If the above range is less than 60%, the space where the slurry stays for coating, that is, the total area between the end of the coating apparatus and the current collector is insufficient compared to the amount of discharged liquid, so that the supplied slurry cannot be coated to leak back. On the other hand, when exceeding 140%, the coating area becomes too large compared to the supplied slurry, resulting in a phenomenon in which coating is performed unevenly.
At the same time, the slurry is discharged from the first discharge port to form a lower slurry layer, and the slurry is discharged again from the second discharge port onto the formed lower slurry layer to form an upper slurry layer. In the present invention, the slurry discharged from the second discharge port is designed to apply a certain level of pressure to the lower slurry layer. Thereby, interlayer interface bondability is improved, and formation of bubbles or the like at the interface is prevented.
In the present invention, the end portions of the lower plate, the middle plate and the upper plate are characterized in that they are located on the same line. In the present invention, the lower slurry layer is first formed through the first discharge port, and then the coating apparatus is moved in the direction opposite to the discharge direction after a certain time has elapsed, thereby securing a space for forming the upper slurry layer through the second discharge port.
In another example, the electrode paste coating apparatus according to the present invention further includes: a first valve for opening and closing discharge of the first discharge port; and a second valve for opening and closing discharge of the second discharge port; and a valve controller for controlling opening and closing of the first valve and the second valve.
Further, the valve controller opens the first valve at the start of the electrode paste application, and opens the second valve when the application apparatus moves in the direction opposite to the discharge direction. It first forms a lower slurry layer by opening a first valve. When the formed lower slurry layer reaches the position of the second discharge port by the movement of the conveyor that moves the current collector, the second valve is opened, and at this time, the upper slurry layer is stably formed on the lower slurry layer. Further, by controlling the opening timing of the first and second valves, the coating start points of the lower and upper slurry layers correspond to each other, whereby the area of the unnecessary portion to be discarded can be minimized.
In another example, for example, at the end of the electrode paste application, the valve controller sets the closing time of the second valve to be a closing delay time delayed from the closing time of the first valve according to the following equation 2:
[ equation 2]
The upper slurry discharge delay time (sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD).
The turn-off delay time according to the above formula 2 minimizes the area of the surplus portion at the coating end time point within a range that does not interfere with the stable formation of the two active material layers.
By the valve-closing delay as described above, the distance difference between the redundant portion, i.e., the coating end point of the upper slurry layer and the coating end point of the lower slurry layer, is adjusted to be within 3 mm. This is because if the length of the surplus portion exceeds 3mm as described above, the area to be discarded increases, which is uneconomical.
In another embodiment, the average thickness (D) of the lower slurry layer formed by the slurry discharged through the first discharge port 1 ) Average thickness (D) of upper slurry layer formed with slurry discharged through the second discharge port 2 ) Ratio of (D) 1 ：D 2 ) In the range of 1: 3 to 3: 1. the thickness ratio is a relative average of the lengths of the respective layers in the thickness direction.
The thickness of the slurry layer as described above can be regarded as the pressure of the slurry supplied immediately. When the pressure of the supplied upper slurry exceeds 3 times of the pressure of the lower slurry layer, the ratio of the thickness of the lower slurry layer to the thickness of the upper slurry layer is 1: 3 or higher, since the upper layer has a stronger pressure than the lower layer, the lower layer slurry may be pushed back in a direction opposite to the coating direction, thereby increasing the possibility of leakage, and the lower slurry may not be properly supplied due to the high pressure of the upper slurry. Further, due to the high pressure of the upper slurry, the supply of the slurry to the lower slurry layer is not uniform, and thus it is difficult to form the lower slurry layer uniformly.
On the other hand, when the pressure of supplying the lower slurry layer exceeds the pressure of the upper slurry layer by 3 times, the ratio of the thicknesses of the lower slurry layer and the upper slurry layer is 3: 1 or higher, there is a problem that the supply of the upper slurry layer becomes difficult, or the coating of the upper slurry layer may be pushed in the coating direction and the surface of the coating liquid may be uneven.
The invention also provides an electrode slurry coating method using the device. In the following description of the electrode paste coating method, portions overlapping with detailed description or specific numerical range limitations mentioned in the description of the apparatus will be omitted.
The method of coating an electrode paste according to the present invention comprises: forming a lower slurry layer by discharging slurry through a first discharge port onto a current collector moving in a coating direction (MD) using an apparatus 130 for coating electrode slurry, the apparatus 130 including a lower plate 131, a middle plate 132, and an upper plate 133; moving the device in a direction opposite to the discharge direction; and forming an upper slurry layer by discharging the slurry onto the lower slurry layer through a second discharge port positioned spaced apart from the first discharge port downstream in the coating direction.
In the present invention, the end portions of the upper plate, the middle plate and the lower plate are positioned on the same line.
In one example, in the electrode paste coating method, at a point of time after a certain time has elapsed after the start of the electrode paste coating, the shortest distance between the end of the coating apparatus and the current collector, that is, the height (H1), is from H1 S Variation H1 T ，H1 T Providing space for forming the sizing layer. Therefore, in the electrode paste coating method according to the present invention, the lower paste layer and the upper paste layer are not mixed, and a two-layer structure composed of the lower paste layer and the upper paste layer is stably formed.
For example, the time point at which the coating apparatus moves in the direction opposite to the discharging direction can be calculated by the following formula 1:
[ equation 1]
Moving the switching point (T) dS Sec) (thickness of the intermediate plate (a) (mm) + thickness of the first discharge port (b) (mm))/moving speed of the current collector in the Moving Direction (MD) (mm/sec)).
In the electrode paste coating method according to the present invention, the height (H1) is changed from H1 after the movement switching point calculated by the above formula 1 S Variation H1 T . This is to stably form an upper slurry layer on a lower slurry layer formed after the lower slurry layer is first formed.
In one example, according to the electrode paste coating method of the present invention, when the electrode paste is coated, the discharge of the paste through the first discharge port is started, and when the coating apparatus is moved in the direction opposite to the discharge direction, the discharge of the paste through the second discharge port is started.
In this way, when the formed lower slurry layer reaches the position of the second discharge port by the movement of the conveyor that moves the current collector, the second valve is opened, and at this time, the upper slurry layer is stably formed on the lower slurry layer. In addition, by controlling the opening timings of the first and second valves as described above, the application start points of the lower and upper slurry layers correspond to each other, whereby the area of the unnecessary portion to be discarded can be minimized.
In another example, the shortest distance between the current collector and the end of the coating apparatus before the start of electrode slurry coating (H1) S ) Is controlled in the range of 60% to 140%, preferably 80% to 120%, more preferably 80% to 100% of the average thickness of the lower slurry layer. If the above range is less than 60%, the space where the slurry stays for coating, that is, the total area between the end of the coating apparatus and the current collector is insufficient compared to the amount of discharged liquid, so that the supplied slurry cannot be coated to leak back. On the other hand, in the case of more than 140%, the coating area is too large compared to the supplied slurry, resulting in that the coating cannot be performed uniformly, or only the lower layer and not the upper layer can be coated.
Here, the shortest distance between the end of the coating apparatus and the current collector means a length from straight ends of the upper, middle and lower plates of the coating apparatus to a vertical tangent of the current collector.
The slurry is discharged from the first discharge port to form a lower slurry layer, and the slurry is discharged again from the second discharge port onto the formed lower slurry layer to form an upper slurry layer. In the present invention, the slurry discharged from the second discharge port is designed to apply a certain level of pressure to the lower slurry layer. Thereby, interlayer interface bondability is improved, and formation of bubbles or the like at the interface is prevented.
In another example, the electrode paste coating method according to the present invention is characterized in that, at the end of electrode paste coating, the discharge stop time of the paste forming the upper paste layer is delayed from the discharge stop time of the paste forming the lower paste layer by a turn-off delay time according to the following formula 2:
[ equation 2]
The upper slurry discharge delay time (sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD).
The turn-off delay time according to the above formula 2 minimizes the area of the surplus portion at the coating end time point within a range that does not interfere with the stable formation of the two active material layers.
The excess portion as described above is referred to as a discharging section, and refers to a section from a point at which the discharge of the slurry is stopped to reduce the thickness of the slurry layer to an end of the discharged slurry.
This can exhibit an effect of reducing an unnecessary portion discarded as the divided section. This results in improved processing efficiency and reduced manufacturing costs. The discharging section refers to a section from a point at which the discharge of the slurry is stopped to reduce the thickness of the slurry layer to the end (end) of the discharged slurry. Typically, when discharge closure is not delayed or not delayed too much, a discharge section of 5.5mm or more typically occurs.
By the slurry discharge delay in the upper slurry layer as described above, the distance difference between the unnecessary portion, i.e., the coating end point of the upper slurry layer and the coating end point of the lower slurry layer, is adjusted to be within 3 mm. This is because, if the length of the surplus portion exceeds 3mm as described above, the area to be discarded increases, which is uneconomical.
Fig. 3 shows a case where the lower slurry layer 111 and the upper slurry layer 121 are sequentially coated on the current collector moved by the conveyor in the coating direction MD and terminated. By delaying the discharge of the slurry of the upper slurry layer as described above, the distance difference between the application end point (E bottom) of the lower slurry layer 111 and the application end point (E top) of the upper slurry layer 121 can be reduced.
Further, by delaying the discharge of the slurry of the upper slurry layer as described above, the length of the unnecessary portion can be reduced as compared with the prior art. Here, the relief section refers to the total distance from the portion (E terminal) where the thickness of the slurry layer starts to decrease to the end (E top) of the slurry layer.
In the present invention, when E bottom and E top coincide, the length of the dump segment is simultaneously reduced.
In another embodiment, the average thickness (D) of the lower slurry layer formed by the slurry discharged through the first discharge port 1 ) Average thickness (D) of upper slurry layer formed with slurry discharged through the second discharge port 2 ) Ratio of (D) 1 ：D 2 ) In the range of 1: 3 to 3: 1. the thickness ratio is a relative average of the lengths of the respective layers in the thickness direction.
Hereinafter, the present invention will be described in more detail by way of the drawings and examples.
Fig. 1 and 2 are schematic views illustrating an active material slurry coating process using an electrode slurry coating apparatus according to an embodiment of the present invention. Referring to fig. 1, the electrode paste coating apparatus includes a lower plate 131 and an upper plate 133, and a middle plate 132 is interposed between the lower plate 131 and the upper plate 133. The slurry containing the active material, the conductive material, and the binder is fluidly moved along the flow path between the lower plate 131 and the middle plate 132, and the slurry forming the lower slurry layer 111 is discharged through the first discharge port 110. The slurry containing the active material, the conductive material, and the binder is fluidly moved along the flow path between the middle plate 132 and the upper plate 133, and the slurry forming the upper slurry layer 121 is discharged through the second discharge port 120. Further, a conveyor (not shown) for moving the current collector 101 in the coating direction MD is positioned to be spaced apart from the first and second discharge ports 110 and 120 by a predetermined distance.
At this time, the end portions of the lower plate, the middle plate, and the upper plate of the coating apparatus are located on the same line.
Further, referring to fig. 2, in the coating apparatus, the end portions of the apparatus, i.e., the end portions of the lower plate, the middle plate, and the upper plate, are spaced apart from the current collector 101 by a predetermined distance. Here, before starting coating, the end of the coating apparatus is spaced apart from the current collector by the shortest distance H1 S 。
The slurry discharged through the first discharge port 110 is formed on the current collector 101 to have an average thickness D 1 And by making the coating apparatus follow and lineAnd a movement controller (not shown) moving in the opposite direction, and the coating apparatus is separated from the current collector by a predetermined distance. Thereafter, the slurry discharged through the second discharge port 120 is formed on the lower slurry layer 111 to have an average thickness D 2 The upper slurry layer 121.
(first embodiment)
The positive electrode of the lithium secondary battery was manufactured by the electrode slurry coating apparatus and method shown in fig. 1. Specifically, at the start of electrode slurry coating, the shortest distance H1 between the surface of the current collector 101 moving along the conveyor belt and the end of the coating apparatus S And 80 μm. The slurry is discharged from the first discharge port 110 to form a lower slurry layer. Then, as shown in fig. 2, the height H1 of the coating apparatus is set from H1 in the direction opposite to the discharging direction S Movement H1 T . The time point at which the coating apparatus moves is calculated by the following equation 1. Specifically, the speed at which the current collector 101 is moved by the conveyor is 50m/min, the thickness (a) of the middle plate is 1mm, and the thickness (b) of the first discharge port is also 1 mm. It is applied to the following equation 1:
[ equation 1]
Moving the switching point (T) dS Sec) ((thickness of the middle plate (mm) + thickness of the first discharge port (mm))/moving speed of the current collector in the Moving Direction (MD) (mm/sec).
The sum of the thickness of the middle plate and the thickness of the first discharge port is 2 mm. In addition, the speed (mm/sec) at which the current collector 101 is moved by the conveyor in the Moving Direction (MD) is 50(m/min), that is, 83.3 (mm/sec). If calculated according to equation 1, the time of transmission (T) ds ) Is 2.4x10 -3 (sec), i.e., 2.4ms (milliseconds).
H1 T Is a distance that the coating apparatus moves in the direction opposite to the discharging direction at the above time, and is 60 μm.
The total average thickness (DT) of the two-layer slurry coated by the electrode slurry coating apparatus was about 150 μm. Wherein the average thickness D1 of the lower slurry layer is 90 μm, and the average thickness D2 of the upper slurry layer is 60 μm.
(second embodiment)
The positive electrode of the lithium secondary battery was prepared using the electrode slurry coating apparatus shown in fig. 1. Since the detailed description of the electrode paste coating method is repeated as in the first embodiment, it is omitted.
However, the distance H1 by which the coating apparatus moves in the direction opposite to the discharge direction T I.e. the starting distance, is 90 μm.
The total average thickness (DT) of the two-layer slurry coated by the electrode slurry coating apparatus was about 180 μm. Wherein the average thickness D1 of the lower slurry layer is 90 μm, and the average thickness D2 of the upper slurry layer is 90 μm.
(third embodiment)
The positive electrode of the lithium secondary battery was prepared using the electrode slurry coating apparatus shown in fig. 1. Since the detailed description of the electrode paste coating method is repeated as in the first embodiment, it is omitted.
However, at the end of the electrode paste application, the closing time of the second valve is delayed from the closing time of the first valve by the closing delay time according to the following equation 2. Specifically, the speed at which the current collector 101 is moved by the conveyor is 50m/min, the thickness (a) of the middle plate is 1mm, and the thickness (b) of the first discharge port is also 1 mm. This is applied to the following equation 2:
[ formula 2]
The upper slurry discharge delay time (sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD).
The sum of the thickness of the middle plate and the thickness of the first discharge port is 2 mm. Further, the speed (mm/sec) at which the current collector 101 was moved by the conveyor in the Moving Direction (MD) was 50(m/min), that is, 83.3 (mm/sec). If calculated according to equation 2, the closing delay time is 2.4x10 -3 (sec) or 2.4ms (milliseconds).
Therefore, at the end of the application of the electrode paste, the closing time of the second valve is delayed by 2.4ms from the closing time of the first valve. In this case, in the fabricated electrode, the coating end points of the lower and upper slurry layers 111 and 121 were the same (E top ═ E bottom), and the dispensing length was the distance from the portion (E terminal) where the thicknesses of the upper and lower slurry layers were reduced to the end (E top, E bottom) where the coating was completed, and the measurement result thereof was 4.5 mm.
Generally, the discharge length is formed to be 5.5mm or more, and in the case of the manufacturing according to the third embodiment, by reducing the length of the unnecessary portion, the portion to be discarded is saved, thereby improving the efficiency of the process.
The invention is described above in more detail by means of figures and examples. Therefore, the embodiments described in the specification and the configurations described in the drawings are only the most preferable embodiments of the present invention and do not represent all the technical ideas of the present invention. It should be understood that various equivalents and modifications may be substituted therefor at the time of filing this application.
[ description of reference numerals ]
101: current collector
110: a first discharge port
111: lower slurry layer
120: second discharge port
121: sizing layer
131: lower plate of coating equipment
132: middle plate of coating equipment
133: upper plate of coating equipment
a: thickness of the middle plate
b: thickness of the first discharge opening

Claims (13)

1. An apparatus (130) for coating an electrode paste, the apparatus being composed of a lower plate (131), a middle plate (132), and an upper plate (133), the apparatus comprising:
a first discharge port (110) formed between the lower plate (131) and the middle plate (132) and configured to discharge a slurry forming a lower slurry layer onto a current collector;
a second discharge port (120) formed between the middle plate (132) and the upper plate (133), positioned to be spaced apart from the first discharge port downstream in a coating direction, and configured to discharge a slurry forming an upper slurry layer onto the lower slurry layer on the current collector; and
a movement controller configured to move the apparatus in a direction opposite to the discharge direction,
wherein the ends of the lower plate, the middle plate and the upper plate are positioned on the same line,
wherein at the start of the application of the electrode slurry, the slurry is discharged through the first discharge port, and
wherein the slurry is discharged through the second discharge port when the apparatus is moved in a direction opposite to the discharge direction.
2. The apparatus of claim 1, wherein the movement controller controls a shortest distance H1 between an end of the apparatus and the current collector to satisfy the condition:
[ Condition ]
When a certain time has elapsed after the lower slurry layer is formed, the apparatus is moved in a direction opposite to the discharging direction to form an upper slurry layer on the lower slurry layer, at which time the apparatus is moved by a distance H1 T In the range of 60% to 140% of the average thickness of the sizing layer.
3. The apparatus according to claim 2, wherein a point of time at which the apparatus moves in a direction opposite to the discharging direction is calculated by the following formula 1:
[ equation 1]
The movement switching point (sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/movement speed (mm/sec) of the current collector in the Movement Direction (MD).
4. The apparatus of claim 1, wherein a shortest distance (H1) between an end of the apparatus and the current collector before electrode slurry coating begins (H1) S ) In the range of 60% to 140% of the average thickness of the lower slurry layer.
5. The apparatus of claim 1, wherein the upper and lower slurry layers have an average thickness of 40 to 200 μ ι η.
6. The apparatus of claim 1, further comprising:
a first valve configured to open and close discharge of the first discharge port;
a second valve configured to open and close discharge of the second discharge port; and
a valve controller configured to control opening and closing of the first valve and the second valve.
7. The apparatus according to claim 6, wherein at the end of the electrode paste coating, the valve controller delays the closing time of the second valve from the closing time of the first valve by a closing delay time according to the following equation 2:
[ formula 2]
Sizing discharge off delay time (T) dT Sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD).
8. A method of coating an electrode paste, the method comprising the steps of:
forming a lower slurry layer by discharging slurry through a first discharge port onto a current collector moving in a coating direction (MD) by using an apparatus (130) for coating electrode slurry consisting of a lower plate (131), an intermediate plate (132), and an upper plate (133);
moving the apparatus in a direction opposite to the discharge direction; and
forming an upper slurry layer by discharging slurry onto the lower slurry layer through a second discharge port positioned spaced apart from the first discharge port downstream in the coating direction,
Wherein the ends of the lower plate, the middle plate and the upper plate are positioned on the same line,
wherein at the start of the application of the electrode slurry, the slurry is discharged through the first discharge port, and
wherein the slurry is discharged through the second discharge port when the apparatus is moved in a direction opposite to the discharge direction.
9. The method according to claim 8, wherein the time point at which the apparatus moves in the direction opposite to the discharging direction is calculated by the following formula 1:
[ equation 1]
Moving the switching point (T) dS Sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD)).
10. The method of claim 8, wherein a shortest distance (H1) between an end of the apparatus and the current collector before electrode slurry coating begins (H1) S ) In the range of 60% to 140% of the average thickness of the lower slurry layer.
11. The method according to claim 8, wherein at the end of electrode paste coating, the time for stopping the discharge of the paste for forming the upper paste layer is delayed from the time for stopping the discharge of the paste for forming the lower paste layer by a turn-off delay time according to the following formula 2:
[ equation 2]
The upper slurry discharge delay time (sec) ((thickness (a) (mm) of the middle plate) + thickness (b) (mm) of the first discharge port))/moving speed (mm/sec) of the current collector in the Moving Direction (MD).
12. The method according to claim 11, wherein a difference in distance between an application end point of the upper slurry layer and an application end point of the lower slurry layer is within 3mm according to a discharge delay.
13. The method of claim 8, wherein the average thickness (D) of the lower slurry layer 1 ) And the average thickness (D) of the sizing layer 2 ) The ratio of 1: 3 to 3: 1.
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